The discovery that ordered nanoporous materials can be produced using a surfactant-templated approach has opened up a new era in the synthesis of ordered nanoscale materials.[1±4] Many investigations have explored the preparation of nanoporous materials with novel chemical composition, [5] the fundamental nature of the reaction processes, [6±8] and potential applications, such as catalysis [9±11] and separation technology, [12,13] which is expected to open up further application possibilities. Interest in the structure of the pore network is necessarily concomitant with the formation of different structures, including hexagonal, cubic, and lamellar structures. The liquid-crystal templating approach to these structures is based on a micellar or tubular structure. After templating, the inorganic precursor condenses to form a rigid cast of the underlying liquid crystal, and the organic phase can be removed to leave an inorganic solid composed of a periodic nanoporous structure with uniform diameter and distribution. Although the feasibility of choosing the pore size offers a wide range of possibilities for hosting different molecules, reports on the drug-delivery behavior of ordered nanoporous materials are not abundant and usually involve structural modification. [6] In particular, a systematic drug-delivery study on the porous geometrical shapes of nanoporous materials has yet not been reported.Here we report the smart drug-delivery application of synthesized L 3 -phase (sponge-phase) nanoporous materials in highly controlled drug release, upon integration of a thermoresponsive polymer, poly(N-isopropylacryl amide) (PNIPAm). The L 3 phase is formed by the self-assembly of amphiphilic templates during the formation of nanoporous inorganic materials, and it consists of a three-dimensional random packing of a multiply connected bilayer of the surfactant and cosurfactant that divides the space into two subspaces filled with solvent, based on the liposome structure. The pore size and the distance between the silicate layers in the porous structure were controlled by changing the hydrophilic domain, for example, by varying the amount of water. The aim of this work is to explore a new potential application of the bicontinuous, disordered, L 3 -phase nanoporous structure and its capability of acting as a convenient reservoir for controlled drug release. For this purpose, we introduced indomethacin (IMC), an antipyretic and analgesic drug, into the non-calcined, silicified L 3 gels and L 3 -integrated thermosensitive PNIPAm polymer gels (L 3 -PNIPAm), and subsequently demonstrated the in-vitro drug-release process by a step-wise temperature change.The synthesis of silicified L 3 gels was achieved using a method that was a slight modification of one previously reported, [14] in which the order of mixing of the three components of the L 3 phase was not important, but it was necessary to maintain the correct ratio of hexanol to the surfactant, 1-hexadecyl pyridinium chloride (CPCl), in order to ensure phase purity and stabi...